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Investigation into the Catalytic Roles of Various Oxygen Species over Different Crystal Phases of MnO2 for C6H6 and HCHO Oxidation
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-05-06 , DOI: 10.1021/acscatal.0c00459 Bingbing Chen 1 , Bo Wu 1 , Limei Yu 1 , Mark Crocker 2, 3 , Chuan Shi 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-05-06 , DOI: 10.1021/acscatal.0c00459 Bingbing Chen 1 , Bo Wu 1 , Limei Yu 1 , Mark Crocker 2, 3 , Chuan Shi 1
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Although manganese oxide (MnO2) exhibits excellent activity in various oxidation reactions, especially for volatile organic compound oxidation, the origin of the catalytic activity remains ambiguous and controversial. In this study, four types of MnO2 catalysts with crystal phases corresponding to α-, β-, γ-, and δ-MnO2 were synthesized, and their catalytic properties in HCHO and C6H6 oxidation were studied. α- and γ-MnO2 were found to possess much better activity for C6H6 oxidation than δ- and β-MnO2 catalysts, whereas δ-MnO2 exhibited the best performance for HCHO oxidation as compared with other types of MnO2. Three kinds of oxygen species were discriminated based on their Mn–O bond strength and reducibility. By quantitatively correlating the amount of specific oxygen species with the reaction rates, the catalytic roles of different oxygen species in HCHO and C6H6 oxidation were clarified. With the assistance of isotopic labeling studies, the participation of oxygen species in C6H6 oxidation—which followed a Mars–van Krevelen mechanism—was illuminated.
中文翻译：
MnO 2的不同晶相上各种氧对C 6 H 6和HCHO氧化的催化作用研究
尽管氧化锰（MnO 2）在各种氧化反应中表现出优异的活性，尤其是对于挥发性有机化合物的氧化，但是催化活性的起源仍然是模棱两可和有争议的。在这项研究中，四种类型的MnO 2对应的催化剂与结晶相到α-，β-，γ-和δ-的MnO 2进行合成，并且在HCHO和C其催化性能6 ħ 6氧化进行了研究。α-和γ-MnO的2被发现具有更好的活性对C 6 H ^ 6的氧化比δ-和β-MnO的2种催化剂，而δ-的MnO 2与其他类型的MnO 2相比，HCHO表现出最佳的HCHO氧化性能。根据其Mn–O键的强度和还原性来区分三种氧。通过定量地将特定氧种类的数量与反应速率相关联，阐明了不同氧种类在HCHO和C 6 H 6氧化中的催化作用。在同位素标记研究的帮助下，照亮了Mars-van Krevelen机制遵循的氧物种参与C 6 H 6氧化的过程。
更新日期：2020-05-06
中文翻译：
MnO 2的不同晶相上各种氧对C 6 H 6和HCHO氧化的催化作用研究
尽管氧化锰（MnO 2）在各种氧化反应中表现出优异的活性，尤其是对于挥发性有机化合物的氧化，但是催化活性的起源仍然是模棱两可和有争议的。在这项研究中，四种类型的MnO 2对应的催化剂与结晶相到α-，β-，γ-和δ-的MnO 2进行合成，并且在HCHO和C其催化性能6 ħ 6氧化进行了研究。α-和γ-MnO的2被发现具有更好的活性对C 6 H ^ 6的氧化比δ-和β-MnO的2种催化剂，而δ-的MnO 2与其他类型的MnO 2相比，HCHO表现出最佳的HCHO氧化性能。根据其Mn–O键的强度和还原性来区分三种氧。通过定量地将特定氧种类的数量与反应速率相关联，阐明了不同氧种类在HCHO和C 6 H 6氧化中的催化作用。在同位素标记研究的帮助下，照亮了Mars-van Krevelen机制遵循的氧物种参与C 6 H 6氧化的过程。
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